Modeling Lanthanide Ions in Solution: A Versatile Force Field in Aqueous and Organic Solvents

Duvail, Magali; Moreno Martinez, Diego; Žiberna, Lara; Guillam, Erwann; Dufrêche, Jean-François; Guilbaud, Philippe

doi:10.1021/acs.jctc.3c01162

J. Chem. Theory Comput.

2024

DOI: 10.1021/acs.jctc.3c01162

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Modeling Lanthanide Ions in Solution: A Versatile Force Field in Aqueous and Organic Solvents

Magali Duvail,

Diego Moreno Martinez,

Lara Žiberna

et al.

Abstract: In this paper, we propose a new nonpolarizable force field for describing the Ln 3+ (Ln = lanthanide) series based on a 12-6-4 Lennard-Jones potential. The development of the force field was performed in pure water by adjusting both the ion−oxygen distance and the hydration free energy. This force field accurately reproduces the Ln 3+ hydration properties through the series, especially the coordination number that is hardly accessible using a nonpolarizable force field. Then, the validity and the transferabili… Show more

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Cited by 6 publications

References 70 publications

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Molecular Insights of Separation of Lanthanide Metals from Aqueous Waste by Using Directional Solvent Extraction

Thakare,

Sappidi

2024

Ind. Eng. Chem. Res.

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In this paper, we present atomistic molecular dynamics simulations to understand the directional solvent extraction (DSE) for separating lanthanide metals from aqueous waste. We consider four different lanthanide metals such as lanthanum (La 3+ ), neodymium (Nd 3+ ), europium (Eu 3+ ), and ytterbium (Yb 3+ ) using decanoic acid (DEC) as a directional solvent. We analyze various molecular mass density profiles, intermolecular structural properties, ion dynamic behaviors, and solvation free energy values of metal ions with the variation in temperature (T). We observe strong intermolecular interactions between the lanthanide ions (Ln 3+ −Ln 3+ ) and lanthanide−nitrate (Ln 3+ −NO 3 ) as the temperature increases. The self-diffusion coefficient (D) of all of the metal ions shows a significant rise with an increase in T values. The detailed solvation free energy ΔG solv (kJ/mol) and transfer free energy ΔG transfer (kJ/mol) calculations provide favorable values in the organic and aqueous phases with the rise in T values. The partition coefficient (log P) values indicates favorable separation of lanthanide ions using DEC. Overall, the molecular level findings described in this manuscript provide great insights into the design of the DSE method for the separation of lanthanide metals from aqueous waste.

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Molecular Insights of Separation of Lanthanide Metals from Aqueous Waste by Using Directional Solvent Extraction

Thakare,

Sappidi

2024

Ind. Eng. Chem. Res.

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Fast and Robust Modeling of Lanthanide and Actinide Complexes, Biomolecules, and Molecular Crystals with the Extended GFN-FF Model

Rose,

Bursch,

Mewes

et al. 2024

Inorg. Chem.

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Lanthanides (Ln) and actinides (An) have recently become important tools in biomedical and materials science. However, the development of computational methods able to describe such elements in various environments has not kept up with the pace of the field. Addressing this challenge, this work introduces and showcases an extension of the GFN-FF to An alongside a reparameterization for Ln. This development fills a gap for fast computational methods that are out-of-the-box applicable to large f-element-containing systems with thousands of atoms. We discuss the reparameterization of the charge model and the covalent topology setup and showcase the model through various applications: Molecular dynamics simulations, optimization of Ln-containing biomolecules, and optimizations of several periodic structures. With the presented improvements, GFN-FF is a powerful method that routinely delivers robust and accurate geometries for large Ln/An systems with thousands of atoms.

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Pairing a Global Optimization Algorithm with EXAFS to Characterize Lanthanide Structure in Solution

Summers,

Zhang,

Sobrinho

et al. 2024

J. Chem. Inf. Model.

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Ensemble-average sampling of structures from ab initio molecular dynamics (AIMD) simulations can be used to predict theoretical extended X-ray absorption fine structure (EXAFS) signals that closely match experimental spectra. However, AIMD simulations are time-consuming and resource-intensive, particularly for solvated lanthanide ions, which often form multiple nonrigid geometries with high coordination numbers. To accelerate the characterization of lanthanide structures in solution, we employed the Northwest Potential Energy Surface Search Engine (NWPEsSe), an adaptive-learning global optimization algorithm, to efficiently screen first-shell structures. As case studies, we examine two systems: Eu(NO 3 ) 3 dissolved in acetonitrile with a terpyridine ligand (terpyNO 2 ), and Nd(NO 3 ) 3 dissolved in acetonitrile. The theoretical spectra for structures identified by NWPEsSe were compared to both experimental and AIMD-derived EXAFS spectra. The NWPEsSe algorithm successfully identified the proper solvation structure for both Eu(NO 3 ) 3 (terpyNO 2 ) and Nd(NO 3 )(acetonitrile) 3 , with the calculated EXAFS signals closely matching the experimental spectra for the Eu-ligand complex and showing good similarity for the Nd salt; the better agreement with the ligand-containing structure is attributed to a less dynamic coordination environment due to the rigid ligand. The key advantage of the global optimization algorithm lies in its ability to sample the coordination environment across the potential energy surface and reduce the time required to identify structures from generally a month to within a week. Additionally, this approach is versatile and can be adapted to characterize main-group metal complexes.

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Modeling Lanthanide Ions in Solution: A Versatile Force Field in Aqueous and Organic Solvents

Cited by 6 publications

References 70 publications

Molecular Insights of Separation of Lanthanide Metals from Aqueous Waste by Using Directional Solvent Extraction

Molecular Insights of Separation of Lanthanide Metals from Aqueous Waste by Using Directional Solvent Extraction

Fast and Robust Modeling of Lanthanide and Actinide Complexes, Biomolecules, and Molecular Crystals with the Extended GFN-FF Model

Pairing a Global Optimization Algorithm with EXAFS to Characterize Lanthanide Structure in Solution

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